Characterization of NOx species in dehydrated and hydrated Na- and Ba-Y, FAU zeolites formed in NO2 adsorption

Adsorbed ionic NO_x species formed upon the interaction of NO₂ with dehydrated or hydrated Na- and Ba-Y, FAU zeolites were characterized using FT-IR/TPD, solid state NMR, and XANES techniques. NO₂ disproportionates on both dehydrated catalyst materials forming NO⁺ and NO₃⁻ species. These ionic species are stabilized by their interactions with the negatively charged zeolite framework and the charge compensating cations (Na⁺ and Ba²⁺), respectively. Although the nature of the adsorbed NO_x species formed on the two catalysts is similar, their thermal stabilities are strongly dependent on the charge compensating cations. In the presence of water in the channels of these zeolite materials new paths open for reactions between NO⁺ and H₂O, and NO₂ and H₂O, resulting in significant changes in the adsorbed ionic species observed. These combined spectroscopic investigations afforded the understanding of the interactions between water and NO₂ on these zeolite catalysts.     

A high statistics measurement of the Lambda(+)(c) lifetime

A high statistics measurement of the Lambda(+)(c) lifetime from the Fermilab fixed-target FOCUS photoproduction experiment is presented. We describe the analysis technique with particular attention to the determination of the systematic uncertainty. The measured value of 204.6 +/- 3.4 (stat) +/- 2.5 (syst) fs from 8034 +/- 122 Lambda(+)(c)-->pK(-)pi(+) decays represents a significant improvement over the present world average.     

Complementary control by additives of the kinetics of amorphous CaCO3 mineralization at an organic interface: in-situ synchrotron x-ray observations

The kinetics of biomimetic mineralization at a fatty acid monolayer interface have been measured in situ by synchrotron x-ray reflectivity. The formation of biologically relevant amorphous calcium carbonate films is affected by soluble macromolecules, supersaturation rate of change, and Mg cations. We find that these solution conditions influence mineral film formation in a complementary fashion. Poly(sodium acrylate) extends the lifetime of metastable amorphous calcium carbonate, solution saturation controls the mineral film growth rate, and Mg cations create a longer induction time. This is the first quantification of potentially competitive biomineralization mechanisms that addresses nucleation and growth of the amorphous mineral phases, which are important in biomineralization.     

一维热传导方程热源反问题基于最小二乘法的正则化方法

研究一维热传导方程热源反问题.给出基于最小二乘支持向量机（LS-SVM）求解的半解析表达式,此外还给出一种参数调节方法以及算法稳定性的证明.数值实验表明该方法具有较高的数值精度和稳定性.     

Infrared emissions, visible up-conversion, thermoluminescence and defect centres in Er3Al5O12 phosphor obtained by solution combustion reaction

The Er₃Al₅O₁₂ phosphor powders were prepared using the solution combustion method. Formation and homogeneity of the Er₃Al₅O₁₂ phosphor powders have been verified by X-ray diffraction and energy-dispersive X-ray analysis respectively. The frequency up-conversion from Er₃Al₅O₁₂ phosphor powder corresponding to the ²H_9/2 → ⁴I_15/2, ²H_11/2 → ⁴I_15/2, ⁴S_3/2 → ⁴I_15/2, ⁴F_9/2 → ⁴I_15/2 and the infrared emission (IR) due to the ⁴I_13/2 → ⁴I_15/2 transitions lying at ∼410, ∼524, ∼556, 645–680 nm and at ∼1.53 μm respectively upon excitation with a Ti-Sapphire pulsed/CW laser have been reported. The mechanism responsible for the frequency up-conversion and IR emission is discussed in detail. Defect centres induced by radiation were studied using the techniques of thermoluminescence and electron spin resonance. A single glow peak at 430°C is observed and the thermoluminescence results show the presence of a defect center which decays at high temperature. Electron spin resonance studies indicate a center characterized by a g-factor equal to 2.0056 and it is observed that this center is not related to the thermoluminescence peak. A negligibly small concentration of cation and anion vacancies appears to be present in the phosphor in accordance with the earlier theoretical predictions.     

Enhancing sensitivity of quadrupolar nuclei in solid-state NMR with multiple rotor assisted population transfers

Rotor-assisted population transfer (RAPT) was developed as a method for enhancing MAS NMR sensitivity of quadrupolar nuclei by transferring polarization associated with satellite transitions to the central m=12-->-12 transition. After a single RAPT transfer, there still remains polarization in the satellite transitions that can be transferred to the central transition. This polarization is available without having to wait for the spin system to return to thermal equilibrium. We describe a new RAPT scheme that uses the remaining polarization of the satellites to obtain a further enhancement of the central transition by performing RAPT-enhanced experiments multiple times before waiting for re-equilibration of the spin system. For 27Al (I=5/2) in albite we obtain a multiple RAPT enhancement of 3.02, a 48% increase over single RAPT. For 93Nb (I=9/2) in NaNbO(3) we obtain a multiple RAPT enhancement of 5.76, an 89% increase over single RAPT. We also describe a data processing procedure for obtaining the maximum possible signal-to-noise ratio.     

First observation of the sigma(*+)(c) baryon and a new measurement of the sigma(*+)(c) mass

Using data recorded with the CLEO II and CLEO II.V detector configurations at the Cornell Electron Storage Rings, we report the first observation and mass measurement of the Sigma(*+)(c) charmed baryon, and an updated measurement of the mass of the Sigma(+)(c) baryon. We find M(Sigma(*+)(c))-M(Lambda(+)(c)) = (231.0+/-1.1+/-2.0) MeV, and M(Sigma(+)(c))-M(Lambda(+)(c)) = (166.4+/-0.2+/-0.3) MeV, where the errors are statistical and systematic, respectively.     

High-field NMR using resistive and hybrid magnets

Resistive and resistive-superconducting hybrid magnets can generate dc magnetic fields much higher than conventional superconducting NMR magnets but the field spatial homogeneity and temporal stability are usually not sufficient for high-resolution NMR experiments. Hardware and technique development addressing these issues are presented for high-resolution NMR at magnetic fields up to 40T. Passive ferromagnetic shimming and magic-angle spinning are used effectively to reduce the broadening from inhomogeneous magnetic field. A phase correction technique based on simultaneous heteronuclear detection is developed to compensate magnetic field fluctuations to achieve high spectral resolution.     

Infrared luminescence, thermoluminescence and defect centres in Er and Yb co-doped ZnAl2O4 phosphor

Er and Yb co-doped ZnAl₂O₄ phosphors were prepared by solution combustion synthesis and the identification of Er and Yb were done by energy-dispersive X-ray analysis (EDX) studies. A luminescence at 1.5 μm, due to the ⁴I_13/2 →⁴I_15/2 transition, has been studied in the NIR region in Er and Yb co-doped ZnAl₂O₄ phosphors upon 980 nm CW pumping. Er-doped ZnAl₂O₄ exhibits two thermally stimulated luminescence (TSL) peaks around 174°C and 483°C, while Yb co-doped ZnAl₂O₄ exhibits TSL peaks around 170°C and 423°C. Electron spin resonance (ESR) studies were carried out to identify defect centres responsible for TSL peaks observed in the phosphors. Room temperature ESR spectrum appears to be a superposition of two distinct centres. These centres are assigned to an O⁻ ion and F⁺ centre. O⁻ ion appears to correlate with the 174°C TSL peak and F⁺ centre appears to relate with the high temperature TSL peak at 483°C in ZnAl₂O₄:Er phosphor.     

Infrared emission and defect centres in Er and Yb codoped Y3Al5O12 phosphors

YAG phosphor powders doped/codoped with Er³⁺/(Er³⁺ + Yb³⁺) have been synthesised by using the solution combustion method. The effect of direct pumping into the ⁴I_11/2 level under 980 nm excitation of doped/codoped Er³⁺/Yb³⁺−Er³⁺ in Y₃Al₅O₁₂ (YAG) phosphor responsible for an infrared (IR) emission peaking at ∼1.53 μm corresponding to the ⁴I_13/2→⁴I_15/2 transition has been studied. YAG exhibits three thermally-stimulated luminescence (TSL) peaks at around 140°C, 210°C and 445°C. Electron spin resonance (ESR) studies were carried out to identify the centres responsible for the TSL peaks. The room temperature ESR spectrum of irradiated phosphor appears to be a superposition of two distinct centres. One of the centres (centre I) with principal g-value 2.0176 is identified as O⁻ ion, while centre II with an isotropic g-factor 2.0020 is assigned to an F⁺ centre (singly ionised oxygen vacancy). An additional defect centre is observed during thermal-annealing experiments and this centre (assigned to F⁺ centre) seems to originate from an F-centre (oxygen vacancy with two electrons) and these two centres appear to correlate with the observed high-temperature TSL peak in YAG phosphor.